Apparatus for the separation of mixed gases



F. E. NORTON.

APPARATUS FOR THE SEPARATION OF MIXED GASES.

APPLICATION FlLED JAN.26, 1918- RENEWED JULY 14, I920.

Patented Sept. 28, 1920.

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ITED STATES PATENT OFFICE.

FRED E. NORTON, OF WORCESTER, MASSACHUSETTS, ASSIGNOR T0 JEFFERIES-NORTON CORPORATION, OF WORCESTER, MASSACHUSETTS, A CORPORATION OF DELAWARE.

APPARATUS FOR THE SEPARATION OF MIXED GASES.

Specification of 'Letters Patent. Patented S t 2 8 1929 Original application filed August 31, 1915, Serial No. 48,325. Divided and this application filed January 26, 1918, Serial No. 213,887. Renewed July 14, 1920. Serial No. 396,334.

To all whom it may concern:

Be it known that I, FRED E. NORTON, a citizen of the United States, residing at Worcester, 'in the county of Worcester andv Commonwealth of Massachusetts, have invented anew and useful Improvement in Apparatus for the Separation of Mixed Gases, of which the following, together Wlth the accompanying drawings, is a specification.

The present application is a division of my copending allowed application covering 'a process of separatin mixed gases, Serial No. 48,325, filed ugust 31, 1915. The present invention in common with that of my aforesaid copending appl1cat1on, relates in general to the art of. separating mixed gases, such as air or water gas, nto their constituent elements, and has particular reference to such systems of separation as contemplate a partial separation of the components ofthe gas by liquefaction, and

various steps employed in the application of said principles'to the accomplishment of the desired results, are fully set forth in the following description, and in the annexed claims, reference being had to the accompanying drawing, in which the figure is a diagrammatic illustration of one arrange-v ment of apparatus for carrying out said invention.

it is tobe understood, however, that the practice'ofm invention is not confined to the employment of the herein described, or any other particular arrangement of appa:

ratus, nor to the herein described methodsof utilizing such apparatus, except in so far as specified in the appended claims; the drawings being merely illustrative, and the description being confined, for the sake. of

clearness and brevity, .to a single special case falling within the scope of the aforesaid principles. 7

The condensation of a mixed gas, as is well known, is characterized by the initial formation of a liquid much richer in the less volatile element of the mixture than the mixture itself, the vapor residue being correspondingly richer in the more volatile element of the mixture. Generally in prior systems of separation, this vapor 'res1due, containing a high percentage of the more volatile element, is liquefied independently, and is used to rectify the products of evaporation from' the aforesaid liquid mixturev which contains a high percentage of the less volatile element. In general, the utilization of these two liquefied portions of the mixture in a rectifying column or still involves progressive contact between the ascending vapors from the mixed liquid which is rich in'the less volatile element, and the descending liquid which is rich in the more volatile element, causing the descendingliquid to exchange with the ascending vapors; whereby the liquid becomes richer in the less volatile element and the vapor becomes richer in the more volatile element, and progressively loses the less volatile component.

It is essential to processes operating on the above principle that the entire supply of the mixed gas be condensed; moreover, the external cooling agency, which in one form or another, is an essential element of all liquefaction systems is called upon to extract large quantities of heat from a portion of the mixture, (namely that portion showinga high percentage of the more volatile element) at a temperature almost as low as the'condensing point of the more volatile element, in order to liquefy the same. Energy, in the form of heat, must be supplied to the liquefied portion containing .a high percentage of the less volatile element in order to evaporate the same, and thisis usually accomplished by causing the said portion, rich in the less volatile element, to condense a portion of the partly cooled, incoming original mixture, which must, therefore, be under considerable pressure. Tnothe'rs words, in the ordinary systems, it is necessary to increase the pressure on the unseparated mixture until its boiling temperature is substantially as low as the boiling temperature of the less volatile element, under the pressure conditions prevailing, in the still.

It is characteristic of such prior systems that the pressures of the descending liquid and ascending vapors in the still-are equal;

it is essential, moreover, that the temperatakes place after the pressure prevailing upon both portions of the liquefied mixture has been released. This release of. pressure results in the reevaporation of considerable amounts of both portions of the liquid and, therefore, imposes a serious limitation on the amount of gas capable of being handled by any given apparatus. This reevaporation also diminishes the purity of the product since at the top of the rectifying column s the outgoing more volatile element cannot be drawn off without also takingwith it some of the mixed evaporate produced by the release of pressure upon the liquid used for rectification.

According to the present invention, the inherent defects and difficulties above enumerated are overcome, by the utilization of the principle that a mixture of elements in vapor form may be made to condense progressively, and while condensing, may be made to evaporate a liquid mixtureof the same elements in different proportions, in such a we that the latent heat of evaporation for the second mixture is supplied by the latent heat of condensation of the first mixture; also by taking advantage of the partial separation accompanying the condensation of a mixture to completely purify the escaping products of distillation, as hereinafter particularly set forth. My invention differs essentially from prior systems in that the liquefaction is accomplihhed under low or onl moderately high pres" sures, while the distillation takes place under high pressures.

With reference to the application of these principles to the attainment of the objects hereinbefore mentioned, the diagrammatic illustration of one arrangement of apparatus for carrying out the invention, as shown in the figure, together with the several steps constituting the process of saidinvention will now be described in detail.

-Referring. by way of example. to the accompanying drawing, the mixed gas dealt recipes with in the system, under relatively low compression; enters a passage 1 of a heat interchanger designated as a whole by the numeral 2. By the action of said interchanger, in conjunction with a refrigerating engine 3 through which a portion of the gas in passage 1 may be drawn, a quantity of the mixed gas, in a liquid state, collects at 4 in the lower end of passage 1, in the manner common to systems of this class. Obviously, the gas used in the refrigerating engine 3, or other external cooling agency, may, if desired, be drawn from'the passage 9, hereinafter referred to, of the heat inter-,

boiling point of said more volatile element but below the boiling point of the original mixture.

Another portion of this uncondensed mixed gas, rich in the more volatile 'element, is withdrawn into a coil 5, placed inside the cold end of a passage 6 of the interchanger 2; in said coil 5 the gas undergoes intense cooling by the action of the cold gases exhausted by the refrigerating engine 8, which are returned through said'passage 6. From the coil 5 the cold gases are led by suitable means, here shown as pipe 7, to a coil 3 placed within the upper end of a third passage 9 of the interchanger. By any suitable. means, here shown aspipe 10, said a'ses are thence led into'admixture at 11 wit the liqpid formed at 4, which liquid undergoes su -cooling by the exhaust gases" from engine 3. The resulting mixture at ll-reaches a composition much higher in the more volatile element than the mixture originally condensed at 4t,'since the liquid has been cooled to a temperature corresponding to the boiling point of a liquid rich in the more volatile element, and hence will condense the more volatile element from the bubbles of vapor supplied at 11, as they rise through the liquid, said bubbles reaching the surface in the form of a vapor rich in the less volatile element and hence more easily condensed. The resulting mixture is conveyed to a pump 12. which serves to raiseit to a much higher pressure than that under which liquefaction toolr place, and delivers itinto the For purposes of illustration, it will be assumed that the gas thus acted upon is air, having, as is well known, a composition of approximately eighty parts nitrogen, the more volatile element, and twenty parts oxygen, the less volatile element. It follows, therefore, that the liquid condensed at 4 in the passage 1 of the heat interchanger will have a much higher percentage of oxygen than atmospheric air; for example, this liquid maycontain fifty per cent. of oxygen, and may have its boiling point at 115 degrees centigrade absolute under a pressure of 10 atmospheres, in comparison to a boiling point of 107 degrees centigrade absolute for air, atfithe-same pressure. As a consequence, the vapor remaining uncondensed in the passage 1, which is led through the coils 5 and 8 as heretofore described, may have or per cent. of nitrogen in its composition, with a boiling point above degrees centigrade absolute (the boiling point of pure nitrogen) and below 107 degrees centigrade absolute, at 10 atmospheres pressure By the action of the gases exhausted from the refrigerating engine 3, the liquid rich in oxygen formed at 4 is cooled to a temperature corresponding approximately to the boiling point of a liquid rich in nitrogen; and it will be assumed that this liquid, together with the vapor rich in nitrogen mixed therewith at point 11, has its pressure raised -from 10 atmospheres to 20 atmospheres by the pump 12, before entering the passage 9. In said passage 9, this liquid is warmed by vheatinterchange with the liquid in passage 1; at the level a where liquid is being condensed in passage 1, the liquid in passage 9 may reach a temperature of degrees centigrade absolute. Above this level, the liquid in 9 extracts heat from the mixed uncondensed vapor in passage 1, the temperature rising gradually as hi her levels in the passage 9 are reached. omewhere above the level l, as, for instance, at the level 13, a temperature of 117 degrees centigrade absolute is reached, the boiling point of pure xiitrogen under 20 atmospheres pressure.

ecause of the difference in composition of the fluids in passages 1 and 9, the liquid in 9 being richerin nitrogen than the-vapor which is just about to condense in 1, there will take place in 9, above the level 13, a. partial evaporation with a corresponding partial condensation in 1 at the same level.

This action is due wholly to the diiierence in composition above set forth; it will be seen,

therefore, that the'increase of pressure imparted to the fluid by the pump is limited by this consideration, and also that the external cooling agency is relied upon to effect a considerable portion ofthe work required for condensation of the fluid in 1. The action above described takes lace over a more or less limited range 0 temperature levels above the level 13, it being understood that within this range of levels there is no actual lowering of the temperature in passage 1, since only the latent heat of condensation is withdrawn, and applied to the evaporation of the liquid in passage 9. Finally a level is reached where the evaporation in passage 9 can no longer accomplish condensation in passage 1; above this level the evaporation in passage 9 serves to cool the incoming uncondensed gas in passage 1. Owing to the phenomena characterizing the condensation of mixed gases, the level at which 'condensa tion first occurs in the passage 1 is considerably higher than that at which the original mixture would completely condense; in the present instance, condensation may begin at or near a level 14 where the temperature is about 122' degrees centigrade absolute, the boiling point of pure oxygen under 10 atmospheres pressure.

The liquid in passage 9, at a level 15, for example, may reach a temperature of degrees centigrade absolute, the boiling point of'pure oxygen under 20 atmospheres pressure. 'The vapors from this liquid ascend in the passage 9 and come in contact with the exterior of coil 8. The cold fluid entering coil 8, under a pressure of 10 atmospheres,

has a temperature below 117 degrees centigrade absolute, the boiling point of pure nitrogen at 20 atmospheres; as a consequence, upon the top, or coldest point of said coil, an exterior condensation of pure nitrogen takes place. The liquid thus formed on the exterior of coil 8 gravitates toward the level 15, coming into intimate contact with the vapor rising from said level. The temperature of said liquid rises as the level 15 is approached; in consequence of this, said liquid progressively parts with its nitrogen and extracts oxygen from the rising vapor. The exchange of elements takes place progressively. practically throughout the whole traverse of said liquid, so that it reaches the level 15 as practically pure oxygen; and as the temperature at the top of coil 8 is maintained at a point below the boiling point of pure nitrogen under 20 atmos-.

pheres pressure, any vapor escaping past this pointmust be pure nitrogen, if the amount of vapor withdrawn is not in excess of the capacity of'the apparatus employed to purify. At the same time, sublit stantially pure oxygen is secured at the level a 15, and may be withdrawn through pipe 16,

if desired, or may be evaporated and utilized in counter-current apparatus, as coil 17, to aid in cooling the incoming mixture.

It will be clear that the vapor employed for circulation through the coil 8, in order to produce the rectification above described, need only be cooled by the refrigerating enine to. a temperature of approximately 1 7 egress centigrade absolute, the boiling point of pure nitrogen under atmospheres pressure. When the ordinary systems are employed, to effect the separation of air, it is usually necessary to cool the liquid used for rectification to the boiling point of nitrogen under atmospheric pressure, namely 80 degrees centigrade absolute, and this cooling must be accomplished at the expense of the external cooling agency, thereby greatly reducing the capacity of the apparatus. As before stated, 'this vapor from the coil 8 meets the liquid formed in the passage 1 at 11, and owing to its contact with a sub cooled liquid having a high oxygen content, the vapor is condensed at a higher temperature than if the mixture were of the composition of the residual vapor in passage 1.

It will thus be seen that in dealing with air, the system is dependent upon the reduction of the temperature of the fluid in coil 8, which may contain a considerablepercentage of oxygen, below the boiling or confrom the refrigerating engine 3.

densing point of pure nitrogen, under the greatly increased pressure prevailing in passage 9. It is clear that the amount and composition of the fluid in coil 8 may be varied, and the relation of the pressures prevailing in passages 1 and 9 so adjusted, that the fluid passing through coil 8 may be part liquid, obtained by a partial liquefaction in coil 5 by the evaporation of liquid formed in the cold end of passage 6 by the exhaust In this manner the highest efliciency for the system is obtainable, since in this part of the apparatus the interchange of heat is caused to take place without change in temperature of the fluid which gives up heat or the fluid which absorbs heat; in other words, the heat exchange results only in condensation and evaporation. In order to obtain this result, it is suflicient that the vapor in coil 5 contain a slightly higher proportion of oxygen than the vapor passing into the refrigerating engine 3,.thereby making it possible to condense aconsiderable amount of the vapor in coil 5 by the evaporation of liquid formed at low pressure in the cold end of passage 6.

' It will be clear, that the system described above, by Way of example, for the separation of. air into its component elements, is

applicable in all aspects to the separation of other mixed gases, many of which possess properties which tend to a more favorable application of the steps of the process than It. is to be under'stoodthat the invention, as hereindescribed, does not of necessity entail either the'complete or the absolute liquefaction of the mixed gaseous fluid which is being separated, and that the terms liquefaction,? liquid and liquefied, as used herein and in the appended claims, apply as Well to a condition of the fluid where in density and temperature it substantially approaches the liquid state. In such a condition said fluid is susceptible, as will be well understood, to a pressure increase by the expenditure of an almost negligible amount of power.

In the applicaion of the new principles underlying the present system, which differ radically and, essentially from the principles underlying previous systems of this class, it is to be understood that my invention is in no sense limited to the equivalents of the apparatus here shown, said showing being wholly diagrammatic and illustrative, and adopted solely for the purpose of simplifying the explanation of said broadly new principles.

I claim,

1. A system of the class described, for separating mixed gases by progressive liquefaction and rectification, comprising a re; verse flow interchanger providing a rectifying column, and means for maintaining a pressure in said column higher than the pressure at which liquefaction of the gas takes place.

2. A system of the class described, for separating mixed ases byprogressive liquefaction, and recti cation, comprising a reverse flow interchanger providing a rectifying column, means for maintaining a pressure in said column higher than the pressure at which liquefaction of the gas took place, and means for rectifying the high pressure vapor in said column by a low pressure fluid containing the same elementsin different proportions.

3. A system of the class described, for the separation of a mixed gas by progressive liquefhction and rectification, comprising a reverse flow interchanger providing a rectifying column, means for sustaining the pressure on the fluid in said column, a coil in said column for the circulation of the vapor residue of progressive liquefaction, and means for mixing said vapor with the liquid passing to the pump.

4. In-apparatus for the'separation of a mixed gaseous fluid, a rectifying column, and means for sustaining the pressure on said fluid during its rectification in said column. I

5. In. apparatus of the class described, means for progressivel 'liquefying a mixed gaseous fluid, means or chilling the residue from said progressive liquefaction,

andmeans for rectifying the va or from the liquefied portion of said'flui by said chilled residue.

6. In apparatus of the class described, means for progressively liquefying a mixed gaseous fluid, means for chilling the residue from said progressive li uefaction, means for rectifying the vapor rom the liquefied portion of said fluid by said chilled residue,

and means for condensing said residue in said liquefied portion.

7. In apparatus of the class described, means for progressively liquefying a mixed gaseous fluid, means for chilling the residue from said progressive. liquefaction, means for raising the pressure on the liquefied portion of said fluid, and means for rectifying the vapor from said liquefied portion, under increased pressure, by said chilled residue.

8. In apparatus for the separation of a mixed gaseous fluid, a rectifying column, and means for circulating therein, in heat exchanging relation to the fluid undergoing rectification, a fluid under lower pressure.

9. In apparatus for the separation of a mixed gaseous fluid, a rectifying column, and means for circulating therein, in heat .exchanging relation to the fluid undergoing rectification, a fluid containing a mixture of the same elements 1n different proportions.

10. In apparatus for the separation of a mixed gaseous fluid, a rectifying column, and means for circulating therein, in heat exchanging relation to the fluid undergoing I liquefaction to said sub-cooled liquid.

13. In apparatus of the class described, means for progressively hquefymg a mixed gaseous fluid, means for chilling the vapor residue from said progressive liquefaction,

means for circulating said chilled vapor residue through the vapor from the liquefied portion of the fluid, to rectify the latter, and means for returning said vapor residue for admixture with said liquefied portion.

14. In apparatus of the class described, means for progressively liquefying a mixed gaseous fluid, means for chilling the vapor residue from said progressive liquefaction, means for increasing the pressure of said liquefied portion, means for circulating said chilled vapor residue through the vapor from said liquefied portion, under increased ressure, to rectify said vapor, and means for returning said vapor residue for admixture with a portion of the liquefied fluid previous to the raising of the pressure thereon.

15. In apparatus for the separation of a mixed gaseous fluid, means for'liquefying a portion of the mixture under low pressure by the evaporation of another portion under higher pressure, said second portion containing a higher percentage of the more volatile component of the mixture than said first portion.

16. In apparatus for the separation of a mixed gaseous fluid, a rectifying column, means for evaporating 'the liquefied fluid in said column, and acoil in said column for the circulation of a fluid having a lower pressure than said evaporate.

17. In apparatus for the separation of a mixed gaseous fluid, a rectifying column,

'means for evaporating the liquefied fluid in said column, and a coil in said column for the circulation of a fluid havlng a lower temperature than said evaporate.

18. In apparatus for the separation of a mixed gaseous fluid, a rectifying column, means for evaporating the liquefied fluid in said column, and a coil in said column for the circulation of a fluid having-a lower pressure and temperature than said evaporate.

19. In apparatus for the separation of a mixed gaseous fluid, means for liquefying a portion of the mixture by the evaporation of anotherportion, said second portion containinga higher percentage of the more volatile component of the mixture than said first portion.

20. In apparatus of the class described, means for liquefying a mixed gaseous fluid, and means for separating and rectifying the same without releasing the pressure thereon.

21. In apparatus of the class described, means for liquefying a mixed gaseous fluid, means for evaporating said liquefied fluid, means for rectifying and separating said evaporate, and means for sustaining pressure thereon during rectification and separation.

. Dated January 22, 1918.

FRED E. NORTON.

Witnesses:

NELLIE WHALEN, PENELOPE COMBERBACH. 

